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Catalytic activity of OH functionalized N-doped graphene in oxygen reduction reaction for fuel cell applications: a DFT study

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Abstract

Catalytic behavior of metal-free hydroxyl group (OH) functionalized single nitrogen (N-Gra(OH)16) and triple nitrogen (N3-Gra(OH)16) doped graphene surface are investigated in the 4e− reduction pathway under oxygen reduction reaction (ORR) process. The thermodynamical parameters indicate that the reaction is highly exothermic and feasible with the N-Gra(OH)16 and N3-Gra(OH)16 as catalysts. However, N3-Gra(OH)16 exhibits better catalytic properties than N-Gra(OH)16. The chemisorption of all reactive species (*O2, *OOH, *O and *OH) via a covalent bond on the N3-Gra(OH)16 and the physisorption of the product H2O on the N3-Gra(OH)16 are essential for efficient reaction kinetics and the uninterrupted reaction cycle, respectively. Categorically, due to the presence of a large number of nitrogen atoms, the N3-Gra(OH)16 exhibits excellent catalytic activity which has resulted in lowered EHOMO–LUMO gap, concomitantly increasing the surface's reactivity. Besides the above, the barrier energies are comparable with platinum (Pt) catalysts. Our results show that the N3-Gra(OH)16 surface is the most suitable catalyst for ORR activity.

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Funding

Thangaraj Thiruppathiraja would like to thank the Department of Science and Technology, New Delhi, India, for providing the financial support [DST-PURSE (II) Fellowship/2020/407].

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  1. Department of Physics, Bharathiar University, Coimbatore, Tamil Nadu, 641 046, India

    Thangaraj Thiruppathiraja & Senthilkumar Lakshmipathi

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339_2023_6464_MOESM1_ESM.doc

The possible structures with nitrogen in the edge positions, Mulliken charge analysis for N-Gra(OH)16 and N3-Gra(OH)16, the HOMO and LUMO plots, the optimized structures of N-Gra(OH)16 and N3-Gra(OH)16 with adsorbate species in the initial state (IS), transition states (TS), intermediates (IM), and final state (FS) phases and their corresponding bond lengths, the relative energy profile of ORR steps, the IRC plot of ORR reactions, the adsorption site for N-Gra(OH)16 and N3-Gra(OH)16 with ORR species, thermochemical properties of the oxygen reduction reaction calculated at M06/6-31G(d,p) level of theory, the calculated electron density and Laplacian of electron density, the rate-limiting step, minimum free energy and overpotential are calculated are given in the Supplementary Information

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Thiruppathiraja, T., Lakshmipathi, S. Catalytic activity of OH functionalized N-doped graphene in oxygen reduction reaction for fuel cell applications: a DFT study. Appl. Phys. A 129, 218 (2023). https://doi.org/10.1007/s00339-023-06464-w

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